Nanomaterials 12 01027

nanomaterials
Review
Metamaterials and Metasurfaces: A Review from the
Perspectives of Materials, Mechanisms and
Advanced Metadevices
Adnan Ali 1 , Anirban Mitra 2 and Brahim Aïssa 1, *
1 Qatar Environment and Energy Research Institute (QEERI), Hamad Bin Khalifa University (HBKU),
Qatar Foundation, Doha P.O. Box 34110, Qatar; adali@hbku.edu.qa
2 Department of Physics, Indian Institute of Technology Roorkee, Roorkee 247667, India;
anirban.mitra@ph.iitr.ac.in
* Correspondence: brahim.aissa@mpbc.ca or baissa@hbku.edu.qa
Abstract: Throughout human history, the control of light, electricity and heat has evolved to become
the cornerstone of various innovations and developments in electrical and electromagnetic technolo-
gies. Wireless communications, laser and computer technologies have all been achieved by altering
the way light and other energy forms act naturally and how to manage them in a controlled manner.
At the nanoscale, to control light and heat, matured nanostructure fabrication techniques have been
developed in the last two decades, and a wide range of groundbreaking processes have been achieved.
Photonic crystals, nanolithography, plasmonics phenomena and nanoparticle manipulation are the
main areas where these techniques have been applied successfully and led to an emergent material
sciences branch known as metamaterials. Metamaterials and functional material development strate-
gies are focused on the structures of the matter itself, which has led to unconventional and unique

electromagnetic properties through the manipulation of light—and in a more general picture the
Citation: Ali, A.; Mitra, A.; Aïssa, B.
electromagnetic waves—in widespread manner. Metamaterial’s nanostructures have precise shape,
Metamaterials and Metasurfaces: A
geometry, size, direction and arrangement. Such configurations are impacting the electromagnetic
Review from the Perspectives of
Materials, Mechanisms and
light waves to generate novel properties that are difficult or even impossible to obtain with natural
Advanced Metadevices. materials. This review discusses these metamaterials and metasurfaces from the perspectives of
Nanomaterials 2022, 12, 1027. https:// materials, mechanisms and advanced metadevices in depth, with the aim to serve as a solid reference
doi.org/10.3390/nano12061027 for future works in this exciting and rapidly emerging topic.
Academic Editors: Julian Maria

Keywords: metamaterial; metasurface; metadevice; plasmonic; nanoparticle; photonic; crystal;
Gonzalez Estevez and José
Antonio Sánchez-Gil
lithography; electromagnetic wave; nanostructure
Received: 30 December 2021

Accepted: 11 February 2022
Published: 21 March 2022 1. Introduction to Metamaterials
Publisher’s Note: MDPI stays neutral Metamaterials are amongst the advanced materials made up initially with metal struc-
with regard to jurisdictional claims in tures. However, there is a huge ongoing work on dielectric metasurfaces and metamaterials
published maps and institutional affil- with the aim of replacing metal structures with dielectric ones in order to reduce the
iations. electromagnetic losses.
Metamaterials’ physical properties rely mostly on their structures. In 1968, Veselago [1]
explored materials of negative permittivity and permeability. Such characteristics though
are not present in naturally found materials and can only be generated in metamaterials.
Copyright: © 2022 by the authors.
During the electromagnetic wave transmission such as wave propagation, the effects
Licensee MDPI, Basel, Switzerland.
generated by metamaterials can be clearly observed. Evolution of the topic of metamaterials
This article is an open access article
distributed under the terms and
with time is presented in Figure 1. From an applications point of view, metamaterials could
conditions of the Creative Commons
be used in devices such as antennas [2], photonic filters [3], integrated network sensors [4]
Attribution (CC BY) license (https:// or new superlayers for the microwave and terahertz fields [5]. The deep understanding
creativecommons.org/licenses/by/ of metamaterials offers fullness of novel options ranging from laboratories concepts to
4.0/). practical engineering applications.
Nanomaterials 2022, 12, 1027. https://doi.org/10.3390/nano12061027 https://www.mdpi.com/journal/nanomaterials

an engineered material intended to attain unique properties and capabilities which are
absent in natural materials. The term metamaterial is introduced by Walser in 1999 [6].
Metamaterial cannot be obtained from any continuous and homogenous medium, that is
why the metamaterials are always of a composite nature. Usually, metamaterials are con-
structed from discrete resonant micro- and nanometer-scale objects which mimic the elec-
Nanomaterials 2022, 12, 1027 tromagnetic reaction of atoms and molecules of natural substances to make them interact
2 of 32
with light and other forms of energy in specific controllable ways.
Figure
Figure 1.
1. Schematic
Schematic depicting
depicting the
the evolution
evolution of
of the
the field
field of
of metamaterials
metamaterials over
over the
the years,
years, from
from 1968
1968
to nowadays.
to nowadays.
2. Classification of Metamaterials
The term “metamaterial” comesAccording
from the to Their
Greek Physical
words Properties
“meta” and “material”, while
“meta”Therefers to something
core concept that is beyond
of metamaterial designusual,
is to rearranged, changed
craft materials or artificially
by using innovative.de- It
is an engineered
signed material
and fabricated intended
structural to attain
units unique
to achieve theproperties and capabilities
desired properties which are
and functionali-
absent
ties. in natural
These materials.
structural units—theTheconstituent
term metamaterial
artificial is introduced
‘atoms’ by Walser of
and ‘molecules’ in the
1999 [6].
met-
Metamaterial cannot be obtained from any continuous and homogenous medium,
amaterial—can be tailored in shape and size, the lattice constant and interatomic interac- that
is why
tion canthe metamaterials
be artificially tuned,are always
and of acan
‘defects’ composite
be designednature.
and Usually,
placed atmetamaterials
desired locations.are
constructed from discrete resonant micro- and nanometer-scale objects which
By engineering the arrangement of these nanoscale unit cells into a desired architecture mimic the
electromagnetic
or geometry, onereaction
can tuneofthe atoms and molecules
refractive index of the ofmetamaterial
natural substances to make
to positive, them
near-zero
interact with light and other forms of energy in specific controllable ways.
2. Classification of Metamaterials According to Their Physical Properties

The core concept of metamaterial design is to craft materials by using artificially
designed and fabricated structural units to achieve the desired properties and function-
alities. These structural units—the constituent artificial ‘atoms’ and ‘molecules’ of the
metamaterial—can be tailored in shape and size, the lattice constant and interatomic inter-
action can be artificially tuned, and ‘defects’ can be designed and placed at desired locations.
By engineering the arrangement of these nanoscale unit cells into a desired architecture or
geometry, one can tune the refractive index of the metamaterial to positive, near-zero or
negative values. By taking into account the permittivity (ε) [7] and permeability (µ) [8] of a
homogeneous material, the metamaterial classification was introduced by Veselago [1]. As
or negative values. By taking into account the permittivity (ε) [7] and permeability (μ) [8]
of a homogeneous material, the metamaterial classification was introduced by Veselago
[1]. As a consequence, some abnormal physical phenomena occur if ε and μ are simulta-
Nanomaterials 2022, 12, 1027 3 of 32
neously negative, such as the reversal of the Snell Law [9], the reversal of the Cherenkov
Effect [10], and the reversal of the Doppler Shift [11]. The relation between the refractive
index (n), ε and μ component parameters are as follows:
a consequence, some abnormal physical phenomena occur if ε and µ are simultaneously
n=
negative, such as the reversal of the Snell Law ±√μ
[9], ε
the reversal of the Cherenkov Effect [10], (1)
and the reversal of the Doppler Shift [11]. The relation between the refractive index (n), ε
andμµ component
and ε are parameters
the material arerelative permittivity and permeability, related to the free
as follows:
space permittivity and permeability by ε = = 8.854 × 10−12 F/m and μ = 4π ×
√
n=± µr ε r (1)
10−7 H/m, respectively. From Equation (1), the value of refractive index “n” depends on
the respective
µr and εr pairs signs εrelative
are theofmaterial and μpermittivity
. For example, flat lens withrelated
and permeability, an isotropic materials
to the free
εrspace
= μr =permittivity
−1 (refractive index n = −1). Therefore, ε the light transmission
and permeability by εo = εr = 8.854 × 10 − 12 F/m and µo = µ = 4π × from
of the radiation
µr
an10object
−7 H/m, is unity for all From
respectively. Fourier components,
Equation even of
(1), the value including
refractiveevanescent waves that
index “n” depends on carry
the
the respective pairs of signs εr and µr . For example, flat lens with an isotropic materials form a
information of high spatial frequency. In other words, flat lens can in principle
perfect
εr = µr image of a point
= −1 (refractive source.
index n = −The classification
1). Therefore, based
the light on the pair
transmission sign
of the ε and from
radiation μ is shown
inanFigure
object 2.
is Various
unity for metamaterials were developed
all Fourier components, with evanescent
even including each quadrant waves corresponding
that carry to
the information
the structure. of high spatial frequency. In other words, flat lens can in principle form a
perfect
Bothimage of a point
parameters source.
ε and Thepositive
μ are classification based on
in quadrant the pair
I and sign ε andasµdouble
are referred is shown positive
in Figure 2. Various metamaterials were developed with each quadrant corresponding to
(DPS) or right-handed medium (RHM). Quadrant I materials are present in nature such
the structure.
as dielectric materials in which propagation of electromagnetic waves can take place. In
Both parameters ε and µ are positive in quadrant I and are referred as double positive
quadrant II, where ε < medium
(DPS) or right-handed 0 —negative, (RHM). and μ > 0—positive,
Quadrant I materialsthe arecorresponding
present in nature materials
such are
known as epsilon
as dielectric negative
materials in which (ENG) medium,
propagation and are represented
of electromagnetic waves can by take
an electric
place. In plasma,
which
quadrantsupport evanescent
II, where waves. Such
ε < 0 —negative, and µmedium has athe
> 0—positive, frequency typically
corresponding between
materials are 2 and
20known
MHz.as Inepsilon
many metals,
negativethe negative
(ENG) medium,value andofare
therepresented
electric permittivity occurs
by an electric below the
plasma,
which support
plasma frequency evanescent waves.frequency
at the optical Such medium has For
range. a frequency typically between
the frequencies lying below 2 andthe me-
20 MHz.
dium In many
frequency, themetals,
real partthe of
negative
electricvalue of the electric
permittivity permittivity
is negative occurs below
and dominates the imag-
inary part. The geometrical parameters of the structure determine the lying
the plasma frequency at the optical frequency range. For the frequencies valuebelow
of medium
the medium frequency, the real part of electric permittivity is negative and dominates
frequency [12]. The quadrant III, where ε < 0—negative, and μ < 0—negative, is known as
the imaginary part. The geometrical parameters of the structure determine the value of
double
medium negative
frequency (DNG) or quadrant
[12]. The left-handed medium
III, where (LHM), andand
ε < 0—negative, doµnot exist in nature.
< 0—negative, is In
quadrant
known asIV, where
double ε > 0 —positive,
negative and μ < 0—negative,
(DNG) or left-handed medium (LHM), theandcorresponding
do not exist in materials
nature. are
termed as μ—negative (MNG), and represented by ferrite materials.
In quadrant IV, where ε > 0 —positive, and µ < 0—negative, the corresponding materials In regions I and III,
most wavesascan
are termed propagate,
µ—negative whereas
(MNG), in regions II
and represented byand IV,materials.
ferrite evanescent wavesI can
In regions be found
and III,
most
and arewaves can propagate,[13–17].
non-propagating whereas in regions II and IV, evanescent waves can be found
and are non-propagating [13–17].
Figure
Figure2.2.Summary
Summary ofofthe
themetamaterial’s
metamaterial’s classification
classification basedbased onpermittivity
on their their permittivity (ε) and permea-
(ε) and permeabil-
bility (μ).
ity (µ). Adapted
Adapted from
from Ref.Ref.
[16].[16].
Nanomaterials 2022, 12, x FOR PEER REVIEW 4 of 33
Thedimensionality
The dimensionalityofof thethe range
range of components
of components that that
formform the (3D)
the bulk bulkstructures
(3D) structures
is
another criterion for metamaterial classification. They are structures that havehave
is another criterion for metamaterial classification. They are structures that a large
a large
number of
number ofconstituent
constituentelements
elements inin any
any given
given direction.
direction. TheThe materials
materials on surface
on the the surface
(i.e., (i.e.,
2D) are equivalent to the case where a thin film structure is made of 1–3 constituents only. only.
2D) are equivalent to the case where a thin film structure is made of 1–3 constituents
Surface-typemetamaterials
Surface-type metamaterialsare aregenerally
generallycalled
called metafilms
metafilms or or metasurfaces.
metasurfaces. Optical
Optical waveg-
wave-
uide with nano inclusions and plasmonics and polaritonic nano-chains
guide with nano inclusions and plasmonics and polaritonic nano-chains are considered are considered
as linear
as linear (1D)
(1D) structures.
structures.AsAsa amattermatter of of fact,
fact, optical
optical waveguides
waveguides are are
alsoalso identified
identified as as
meta-waveguides[18–20].
meta-waveguides [18–20].
Metamaterialsinina afunctional
Metamaterials functionalapplications
applications field
field were
were extensively
extensively investigated,
investigated, and and
included(but
included (butnot
notlimited
limited to)to) light
light sources,
sources, sensors,
sensors, memory,
memory, phasephase
change,change, microelec-
microelectro-
tromechanical
mechanical systems
systems (MEMS),
(MEMS), nanoelectromechanical
nanoelectromechanical systems
systems (NEMS),
(NEMS), superconductors
superconductors
(based onon negative
negative index
indexmetamaterials),
metamaterials),chiralchiralmetamaterials
metamaterials(intrinsic
(intrinsicand
andextrinsic
extrinsicmeta-
metasurfaces), dispersion
surfaces), dispersion metamaterials
metamaterials andand artificialmagnetism
artificial magnetismand and transformation
transformation op- optical
tical metamaterials [14,15,21,22].
metamaterials [14,15,21,22].
The
Theterm
termmetamaterial
metamaterialisisalso alsoused in in
used conjunction
conjunction with artificially
with designed
artificially materials
designed materials
to exhibit
exhibit novel properties of waves such as phononic metamaterials [23]. the
novel properties of waves such as phononic metamaterials [23]. On On other
the other
hand,
hand, electromagnetic
electromagneticwaves wavesare arestimulated
stimulated bybya different kind
a different of non-electromagnetic
kind of non-electromagnetic
waves such
waves suchasasthe sound
the soundwaves of piezoelectric
waves and/orand/or
of piezoelectric spin waves
spinofwaves
nanostructured mag-
of nanostructured
netic materials.
magnetic materials.
3. Evolution
Evolutionof ofMetamaterials
Metamaterials
In
In 2019, Vicarietetal.
2019, Vicari al.[24]
[24]modeled
modeledthe thegrowth
growth of of
metamaterial-containing
metamaterial-containing devices
devices
across eight different applications (displayed in Figure 3). The model looked
across eight different applications (displayed in Figure 3). The model looked at potential at potential
addressable
addressable markets
marketsbased
basedon onvarious
variousparameters
parametersincluding
includingthe thecost,
cost,maturity
maturity and per-
and perfor-
formance. It is based on inputs from a wide range of primary and secondary
mance. It is based on inputs from a wide range of primary and secondary research. Vicari research.
Vicari
and hisand hisexplicitly
team team explicitly
seizedseized the markets
the markets for metamaterial
for metamaterial components
components in commu-
in communications,
nications, sensing and acoustic applications. Many other applications
sensing and acoustic applications. Many other applications are likely to appear are likely to appear
and were
and were grouped together into an “other” category. Market forecast for
grouped together into an “other” category. Market forecast for metamaterials is put metamaterials is at
put atbillion
$10.7 $10.7 billion by Through
by 2030. 2030. Through2025, 2025, communications
communications usesuses arefar
are by by the
far leading
the leading
growth
growth driver; however, by 2030, sensing uses grow to be the largest segment, reaching
driver; however, by 2030, sensing uses grow to be the largest segment, reaching $5.5 billion
$5.5 billion compared to $4.4 billion in communications.
compared to $4.4 billion in communications.
Figure 3.
Figure Metamaterialsmarket
3.Metamaterials market forecast:
forecast: metamaterial
metamaterial devices
devices are are poised
poised to grow
to grow to $10.7
to $10.7 billion
billion by by
2030
2030 in
in 5G
5Gnetworks,
networks,autonomous
autonomousvehicles and
vehicles connected
and vehicles.
connected Adapted
vehicles. fromfrom
Adapted Ref. Ref.
[24].[24].
The origin of metamaterials could be linked to various examples of the pyramid brick
wall, Parthenon columns and medieval ruby glass, as shown in Figure 4. Other “historical”

The origin of metamaterials could be linked to various examples of the pyramid brick
wall, Parthenon columns and medieval ruby glass, as shown in Figure 4. Other “histori-
cal” examples
examples of metamaterials
of metamaterials are, are, for instance,
for instance, the the
work work on the
on the rotation
rotation of the
of the polariza-
polarization
tion
planeplane through
through artificial
artificial twisted
twisted structures
structures performed
performed in 1898,
in 1898, andandthethe artificial
artificial dielec-
dielectric
tric structures
structures for microwave
for microwave antennaantenna
lenseslenses
achievedachieved
in 1945. inThe
1945. The modern
modern (formally (formally
named)
named) metamaterial
metamaterial was noticeable
was noticeable when Pendry whenetPendry et al. [25] anticipated
al. [25] anticipated that arrays that arrays of
of conducting
conducting
wire can functionwire can
withfunction with
a negative a negative
value value
of effective of effectiveatpermittivity
permittivity at a frequency
a relatively low relatively
low
(<200frequency (<200 THz),
THz), whereas whereas
the split the split ring
ring resonators resonators
(SRRs) (SRRs) can
can be utilized be utilized
to facilitate to fa-
a strong
magnetic
cilitate resonance
a strong which
magnetic resulted which
resonance in an effective
resultedpermeability
in an effective negative value.negative
permeability In 2000,
by linking
value. bothby
In 2000, structures and overlapping
linking both structures and theoverlapping
negative frequency bands,
the negative a metamaterial
frequency bands,
acarrying a negative
metamaterial refraction
carrying indexrefraction
a negative was presented
index wasfor the first time,
presented forwhere the
the first directions
time, where
of the
the wave vector
directions of theand the energy
wave flux,the
vector and alsoenergy
knownflux, as backwards
also known waves, were opposite
as backwards waves,in
a negative
were oppositeindex
in medium.
a negativeThese
indexexperiments
medium. These haveexperiments
proven the predictions
have proven ofthe
Veselago’s
predic-
1968 negative
tions index materials
of Veselago’s [1], such
1968 negative indexas negative
materialsrefraction,
[1], such Doppler’s
as negative reversed effectDop-
refraction, and
Cherenkov’s reversed radiation [10].
pler’s reversed effect and Cherenkov’s reversed radiation [10].
Figure 4. Examples of some “historical” original metamaterials, adapted from Ref. [26].
Figure 4. Examples of some “historical” original metamaterials, adapted from Ref. [26].
Metasurfaces
Depending
Depending on on the
the materials
materials employed
employed and and geometry,
geometry, andand per
per their
their frequency
frequency re-re-
sponses,
sponses, metasurface-based device’s classification has been made as narrowband [3,27],
metasurface-based device’s classification has been made as narrowband [3,27],
broadband [28–30] and wideband [31]. Fano Fano resonance
resonance isis the typical case of narrowband
application.
application. The
The sharp
sharp resonance
resonance peak
peak complemented
complemented by by strong local field enhancement
is amongst
amongst the most important
important aspects
aspects of Fano resonance [32,33]. It It is the foundation
foundation of
several practical
practicalapplications
applicationssuchsuch as nonlinear
as nonlinear photonics
photonics and biological
and biological sensing.
sensing. Metasur-
Metasurface dispersion
face dispersion for multiband
for multiband and broadband
and broadband applications
applications can support
can support super-res-
super-resolution
imagingimaging
olution beyond the diffraction
beyond limit, high-performance
the diffraction color filter,
limit, high-performance broadband
color absorbers
filter, broadband
and polarizers
absorbers [31,34–36].[31,34–36].
and polarizers
Metasurfaces are two-dimensional
Metasurfaces two-dimensional (2D) or planar versions of metamaterials dealing
with subwavelength
subwavelengththickness
thickness[37–39].
[37–39].Metasurfaces
Metasurfaceshave
haveunique abilities
unique to block,
abilities absorb,
to block, ab-
concentrate, disperse or guide waves on the surface at a grazing incidence
sorb, concentrate, disperse or guide waves on the surface at a grazing incidence angle andangle and in
space at normal and oblique incidence, from microwave to visible frequencies.
in space at normal and oblique incidence, from microwave to visible frequencies. Surface
waves can
waves can be
be well
well controlled
controlled by
by designing
designing impedance
impedance cells
cells to
to manipulate
manipulate phase
phase or or group
group
velocity [40,41]. These are patterned in such a way that may guide or separate waves
in certain directions, and/or used to control scattering. By controlling the metasurface,

velocity [40,41]. These are patterned in such a way that may guide or separate waves in
certain directions, and/or used to control scattering. By controlling the metasurface, unit
cell sizes and shapes, multiple effective surface refractive indices can be achieved and dif-
unit cell sizes and shapes, multiple effective surface refractive indices can be achieved
ferent functions
and different can be patterned
functions on the surface.
can be patterned They canThey
on the surface. be used to used
can be design to2D micro-
design 2D
wave/optical lenses for antenna systems and planar microwave sources, such
microwave/optical lenses for antenna systems and planar microwave sources, such as as Luneburg
and fish-eyeand
Luneburg lenses [42]. lenses [42].
fish-eye
The
The perspective of
perspective current implementation
of current implementationand andgrowing
growingmetasurface
metasurface andand metade-
metadevice
vice developments are shown in Figure 5. Different metasurfaces demonstrate
developments are shown in Figure 5. Different metasurfaces demonstrate different capabili- different
capabilities. The surface
ties. The surface impedance
impedance can be modified
can be modified and controlled
and controlled by the structure
by the structure of the
of the cells that
cells that are widely applied to surface wave absorbers and surface waveguides.
are widely applied to surface wave absorbers and surface waveguides. These metasurfaces These
metasurfaces also enable transmission
also enable transmission and reflectionand reflection
to shape to shape the beam.
the beam.
Chartsummarizing
Figure5.5.Chart
Figure summarizingthe
themetasurfaces’
metasurfaces’and
andmetadevices’
metadevices’applications.
applications.
Three-dimensional(3D)
Three-dimensional (3D)metamaterials,
metamaterials,mademadeoften
oftenwith
withperiodic
periodicartificial
artificialmaterials
materials
composed of metals and/or dielectrics, have been widely studied owing
composed of metals and/or dielectrics, have been widely studied owing to their uniqueto their unique
interactionwith
interaction withelectromagnetic
electromagneticwaves
wavesthat
thatexceed
exceedthe
thecapabilities
capabilitiesofofnaturally
naturallyoccurring
occurring
or homogeneous materials [27,43,44]. Their exceptional ability to manipulate waves isisdue
or homogeneous materials [27,43,44]. Their exceptional ability to manipulate waves due
to their strong interaction with electrical and/or magnetic fields, typically provided
to their strong interaction with electrical and/or magnetic fields, typically provided by by
unit cell geometry-controlled resonant effects. These capabilities result in a broad
unit cell geometry-controlled resonant effects. These capabilities result in a broad range range
ofofapplications
applicationssuch
suchasasantenna
antennaefficiency
efficiencyenhancement
enhancement[45,46],
[45,46],ideal
idealabsorbers
absorbers[47–49],
[47–49],
superlenses [25,50], cloaking [51–53], elimination of scattering [28,54] and energy
superlenses [25,50], cloaking [51–53], elimination of scattering [28,54] and energy harvest- harvest-
ing[16,55,56],
ing [16,55,56],among
among other
other applications
applications ininmicrowave
microwaveand andoptical
opticalfrequencies.
frequencies. When
When active
ac-
and nonlinear components such as transistors [57,58], diodes [58,59], and varactors [60–62]
tive and nonlinear components such as transistors [57,58], diodes [58,59], and varactors
are added to metasurfaces, novel tunability and switching abilities become possible.
[60–62] are added to metasurfaces, novel tunability and switching abilities become possi-
ble.
4. Metamaterial Fabrication Techniques
Transmission
4. Metamaterial line, resonant
Fabrication and hybrid methods are among the most common design
Techniques
approaches to efficiently fabricate metamaterials from a micrometer to nanometer scale.
The Transmission
implementation line,ofresonant and hybrid
hard materials suchmethods are among the into
as dielectrics/metals mostflexible
common design
materials,
approaches
combined withto efficiently fabricate
the cutting-edge metamaterials
nanometer featurefrom
size atechniques,
micrometer tomade
has nanometer scale.to
it possible
fabricate stretchable devices across multidisciplinary.
The implementation of hard materials such as dielectrics/metals into flexible materials,
combined with the cutting-edge nanometer feature size techniques, has made it possible
to fabricate stretchable devices across multidisciplinary.
4.1. Photolithography
4.1.Photolithography
Photolithography is a technique of microfabrication, which can be used to synthesize
metamaterials that work at terahertz frequencies. This technique has been commonly used
Photolithography is a technique of microfabrication, which can be used to synthesize
in the manufacturing
metamaterials of single
that work and multilayer
at terahertz (3D)
frequencies. metamaterials
This technique has[63],
beensince it is able to
commonly
fabricate high-resolution subwavelength structures at wavelength 30 μm –
used in the manufacturing of single and multilayer (3D) metamaterials [63], since it iswith
3 mm able min-
imal complication
to fabricate [64,65]. Figure
high-resolution 6 provides
subwavelength an example
structures of the reported
at wavelength 30 µm–3 mm metamaterial
with
minimal complication [64,65]. Figure 6 provides an example of the reported metamaterial
made by microfabrication onto flexible substrates. Resonators have been fabricated in the
made
metal bydeposited
film microfabrication onto flexible
on spin-coated substrates.
polyimide Resonators
substrates. have been
In order fabricated
to prevent the in
delam-
the metal film deposited on spin-coated polyimide substrates. In order to prevent
ination of metal structures, the micron resolution patterns produced by this technique are the
delamination of metal structures, the micron resolution patterns produced by this technique
typically further coated with a thin film of polyimide. In general, microfabrication photo-
are typically further coated with a thin film of polyimide. In general, microfabrication
lithography techniques
photolithography are only
techniques areappropriate for substrates
only appropriate that are
for substrates thatorganic and corrosive
are organic and
solvent resistant.
corrosive solvent resistant.
Figure
Figure6. (A). Photolithography:
6. (A). Photolithography:Microfabricated
Microfabricatedterahertz
terahertz metamaterials
metamaterials on onflexible
flexiblesubstrates,
substrates, (B)
Shadow MaskMask
(B) Shadow Lithography
Lithography(SML): SML
(SML): SMLmanufacturing
manufacturingsequence,
sequence,(A,B) Reprintedwith
(A,B) Reprinted withthetheper-
permis-
sion of Copyright
mission © 2018,
of Copyright Springer
© 2018, International
Springer PublishingAG).
International Publishing AG). (C)(C) Electron
Electron Beam Beam Lithography
Lithography
(EBL): (a–g)
(EBL): (a–g)Steps
Stepsfor
forthe
thetransferred double-layergraphene
transferred double-layer graphene on on a flexible
a flexible substrate.
substrate. (Reprinted
(Reprinted with with
permission from Elsevier and Copyright Clearance Center), (D) Soft Lithography,
permission from Elsevier and Copyright Clearance Center), (D) Soft Lithography, (a–c) Fabrication of (a–c) Fabrication
of elastomeric stamps,(d–f)
elastomeric stamps, (d–f) Replica
Replica molding
molding (g–i)(g–i) transfer
transfer printing,
printing, (E) Transfer
(E) Transfer Lithography:
Lithography: Flexible Flex-
iblephotonic
photonic metastructures
metastructures (a) schematic
(a) schematic for a high-contrast
for a high-contrast metastructure
metastructure (HCM) preparation.
(HCM) preparation. (b) SEM (b)
SEM images
images after
after etching.
etching. (c) (c) Microscopic
Microscopic (left)
(left) andand
SEMSEM (right)
(right) fortransferred
for the the transferred
HCMs HCMs on PDMS.
on PDMS.
(Reprinted
(Reprinted with
withpermission
permission from RoyalSociety
from Royal Societyofof Chemistry).
Chemistry).
4.2.4.2. Shadow
Shadow MaskLithography
Mask Lithography
The shadow mask lithography (SML) is a technique which is acid-free manufacturing,
The shadow mask lithography (SML) is a technique which is acid-free manufactur-
produces micro- and nanoscale patterns in planar and multiple layers, similar to screen
ing, produces micro- and nanoscale patterns in planar and multiple layers, similar to
printing of conductive ink. This technique involves direct deposition of thin metal films,
screen
oxidesprinting
or otherofdielectric
conductive ink. This
particles technique
on substrate involves
using direct
a pattern deposition
without of thin
any etching andmetal
films, oxides or other
photolithography dielectric
[66–68]. particles on substrate
The manufacturing sequence ofusing a pattern
the SML without
technology any etching
is shown in
and photolithography
Figure [66–68].
6A [69,70]. A stencil The manufacturing
is fabricated sequence
usually by etching of the
the silicon SML
wafer technology is
or aluminum
foil. The stencil is either directly in contact with the substrate or close to it. In order to
exploit its inherent line-of-sight depositing characteristics, required metal or dielectric

layers, primarily by evaporation of the electron beam, are then deposited. Features of
up to 100 nm can be fabricated while using the SML on arbitrary substrates which are
chemically sensitive or mechanically fragile (including plastic and polymeric substrates).
This method permits large area fabrication of nano-patterning. The stencils are reusable,
with high-performance pattern replication showing repeatable results. However, over
repeated cycles of deposition the resolution of the recognized patterns often deteriorate
due to stencil contact and proximity to the substrate during deposition [71].
4.3. Soft Lithography

Soft lithography (SL) is a class of technologies employed to fabricate or reproduce
structures utilizing elastomeric stamps, molds and conformable photomasks. Because it
uses elastomeric materials, most notably polydimethylsiloxane (PDMS), it is called soft.
SL enables the multi-scale patterning on polymers or other substrates of micro/nanoscale
patterns [72]. With high-resolution replica molding, any polymer compliant to the PDMS
stamping, including non-photolithographic definable polymers, can also be patterned with
high resolutions. A free-standing design is developed by fabricating an inverted copy of
the stamp that can be detached from the carrier [70].
The transfer printing is another widely employed manufacturing technique. Charac-
teristics of any required materials such as metals, semiconductors or functional oxides can
be developed on a silicon substrate. It facilitates the application of well-known patterning
technologies. The elastomeric stamp is used to “pick up” the patterns and then transfer to
the substrate. It is useful and simple method but demanding highly monitored precision
to transfer patterns to the target substrate with high adhesion [73]. Figure 6B presents
a 3D modular transfer printing for assembly on universal substrates of heterogeneously
integrated metamaterials/metadevices [73,74].
By using soft lithography techniques, plastic substrates’ limitations such as expansion
at high temperatures, poor adhesion, low processing temperatures and chemical instabilities
are eliminated. These techniques are also applicable to a wide range of structure sizes and
allow non-planar surface patterning.
4.4. Electron Beam Lithography

Electron beam lithography (EBL) utilizes a focused electron beam wavelength at
high accelerated voltages to achieve nanoscale structures (Figure 6C) [75,76]. Similar to
traditional photolithographs where ultraviolet (UV) light is applied to a photo-resistant
substrate, the EBL technique includes exposure by the high-energy electron beam to an
electron beam resist, such as polymethyl methacrylate (PMMA). This leads to a division in
the organic structure, where the area exposed to the e-beam fully dissolves in the developer
solution. Then, metal/or dielectric layers are deposited, and the resist is dissolved to obtain
the nanoscale patterns. The “lift-off” process is used in this technique, which means that
the reverse design defined by the EBL must be the required pattern. In order to create
nanoscale features under the diffraction boundary of the traditional photolithographic
processes, EBL is highly suitable and does not require a physical mask for pattern transfers.
The EBL technology is used for the fabrication of subwavelength resonators. Although
EBL is a powerful technique for achieving nanometer and submicron characteristics, the
development of high-performance large-scale metamaterials must overcome three major
limits, namely the lengthy writing times because technique is serial; periodical stitch errors;
and the lack of stability and potential astigmatism of the electron beam. Furthermore, serial
patterning causes drifting beam instability, and a wide area of many steps is leading to
a poor resolution and stitching defects. Secondly, stitching errors also adversely affect
the reproduction ability of the patterns without a misalignment on a large area. Finally,
the reliability, precision and stigma of electron beam whitening have a decisive effect on
the technique’s efficacy. The blanket beam is an outer voltage source, which is used for
switching on and off electron beams when moving nanoscale functionality. During the
extensive writing times usually associated with this process, any variation will lead to
incoherent exposure and introduces geometric errors [74,77].
4.5. Three-Dimensional Metamaterial Fabrication Techniques

The formation of multiple 3D metamaterials was primarily based on planar processing
techniques. For instance, cloaking [51,52], imaging below diffraction limit [78,79], quantum
levitation and sensing [80] can be successfully achieved by 3D terahertz or optical metama-
terials. However, anisotropic responses often affect such multilayered metamaterials. This
cannot be achieved by planar processes to generate metamaterials with epsilon (ε) and mu
(µ) isotropic negatives. Additional innovations in manufacturing technology have been
pursued such as specific additive production processes, to obtain isotropic response meta-
materials for the subwavelength dimension. Such techniques include imprint lithography,
vertical pillar superlattice, multiphoton polymerisation, electroplating in multilayer, inkjet
printing and interference lithography [74,76,77,81–84].
Many other manufacturing techniques are developed in order to create a 3D split-
ring resonator (SRR) metamaterial, by a combination of laser writing and chemical vapor
deposition techniques [75,85]. Figure 7 shows a heterogeneously integrated metamate-
rial/metadevice assembly on universal substrates by 3D modular transfer printing. The
technique of chemical vapor deposition grows a uniform metal film coating of the structure
that cannot be obtained using other techniques. A focused ion beam (FIB) milling is another
3D manufacturing technique used for the fabrication of features with high aspect ratios at
the nanometer scale [66,86]. The multiple-layer deposition of metal and dielectric layers
was developed to create a 3D fishnet resonator. Etching of high aspect ratio nanometer-sized
features was carried out by FIB milling. Furthermore, plasma etching can be used instead of
the FIB milling. To produce sophisticated negative index metamaterials, a combination of
printing techniques with other large-area lithography techniques can be used. Fabrication
technique using 3D direct laser writing (DLW) may be utilized to fabricate metamaterial
structures with complex geometry [87,88]. The DLW technique involves incident of a firmly
focused laser beam on a diffraction-limited spot inside the photoresist’s volume. This
enables the development of three-dimensional nanometer-scale features that cannot be
manufactured using traditional lithography techniques. Whereas direct writing methods
can reach optimized resolutions, they suffer from low output and are only suitable with a
limited number of substrates. Multiple laser wavelengths technique can further improve
the spatial resolution.
Another sophisticated fabrication technique of producing micrometer-scale 3D meta-
materials is membrane projection lithography (MPL). Typically, this technique employs
a patterned membrane layer built over a cavity to serve as a mask layer to the cavity’s
underlying wall surfaces and bottom surface. A beam may be guided through the template
opening onto the underlying surface, with the opening serving as a mask for regulating the
area of the underlying surfaces on which any implantation occurs. MPL can revolutionize
future 3D infrared and optical metamaterial structures with complex geometries, thanks to
its high degree of control over the design and deposition of thin films [89].
Caputo et al. proposed a completely different approach to achieve hyper-resolution
of a generic two-photon direct laser writing (TP-DLW) lithography process exploiting the
extraordinary collimation of the writing laser light enabled by an optical epsilon-near-
zero (εNZ ) nanocavity in a metal/insulator/metal/insulator (MIMI) configuration [90]. In
particular, the proposed technique reaches its optimum when 2D and 3D complex nanos-
tructures are under consideration. The proposed metamaterial is exploited to successfully
fabricate 1D gratings with a height adjustable from 5 nm to 50 nm. Achieved results
provided the driving force to implement a novel and highly effective approach for devel-
oping ultrathin all-dielectric metalenses. The ground-breaking advantages of this novel
technique include cost effective and time effective single-step fabrication, nanometric sizes
and all-dielectric composition. This technique can be used in applications across industry
Nanomaterials 2022, 12, 1027 developing ultrathin all-dielectric metalenses. The ground-breaking advantages 10 of 32 of th
novel technique include cost effective and time effective single-step fabrication, nanome
ric sizes and all-dielectric composition. This technique can be used in applications acros
industry
and and
scientific scientific
research, research,
such such as in optical
as in miniaturized miniaturized
devices,optical devices,
advanced advanced
microscopy and micros
copy and[87,88,90].
flat-optics flat-optics [87,88,90].
Figure
Figure 7. 7. Heterogeneously
Heterogeneously integrated
integrated metamaterial/metadevice
metamaterial/metadevice assembly assembly onsubstrates
on universal universal bysubstrate
bymodular
3D 3D modular transfer
transfer printing:
printing: (a) modularized
(a) modularized basicblocks
basic building building blocks preparation,
preparation, (b) metamate
(b) metamaterials
rials on a silicon membrane (MoSM) and graphene on a silicon (GoSM) picking up
on a silicon membrane (MoSM) and graphene on a silicon (GoSM) picking up by the 5-microtip stamp. by the 5-microti
stamp. (c) Three-dimensional modular transfer printing used to fabricate a metamaterial/metade
(c) Three-dimensional modular transfer printing used to fabricate a metamaterial/metadevice. Two-
vice. Two-dimensional
dimensional and three-dimensional
and three-dimensional metamaterials andmetamaterials
metadevices byand metadevices
assembling each by assembling eac
individual
building lock (i.e., MoSM or GoSM). (Reprinted with the permission of Copyright © 2018, Springer © 201
individual building lock (i.e., MoSM or GoSM). (Reprinted with the permission of Copyright
Springer International
International Publishing AG).
Publishing AG).
Though
Though these
these techniques
techniques are promising
are promising in creating
in creating 3D metamaterial
3D metamaterial structures;
structures; how- how
ever, they are not versatile and mature enough. Some of these presented methods are
ever, they are not versatile and mature enough. Some of these presented methods are ra rather
complex and need
ther complex andvarious manufacturing
need various steps thatsteps
manufacturing impact their
that structural
impact theirresolution,
structural resolu
while others are restricted by the type of materials employed for the patterning process and
tion, while others are restricted by the type of materials employed for the patterning pro
also by the option of the appropriate substrates. Additionally, transfer techniques are based
cess and also by the option of the appropriate substrates. Additionally, transfer technique
on the chemistry of the surface, and as a result, they are reliant on it. Overall, the use of
are based on the chemistry of the surface, and as a result, they are reliant on it. Overal
the use of complex techniques involving soft lithography and photolithography fusion t
Nanomaterials 2022, 12, x FOR PEER REVIEW

guide the pattern transfer to highly curved substrates remains a technological c
to achieve high-resolution patterns of <0.1 μm.
complex techniques involving soft lithography and photolithography fusion to guide the
pattern transfer to highly curved substrates remains a technological challenge to achieve
5. Emerging Functional Metadevices
high-resolution patterns of <0.1 µm.
Metamaterial research has shifted recently to the so called “integrated metad
5.known
Emerging
as Functional
super cellMetadevices
[91] (Figure 8). Extensive studies have been conducted ou
Metamaterial research has shifted
electromagnetic photonic [52], terahertz recently to the so called
[92] and “integrated
microwave metadevices”,
metamaterials
known as super cell [91] (Figure 8). Extensive studies have been conducted outside the
phase-change devices [93], graphene [94], carbon nanoubes [95], semiconductors
electromagnetic photonic [52], terahertz [92] and microwave metamaterials utilizing phase-
uid crystals
change devices[96].
[93], The ultimate
graphene goal isnanoubes
[94], carbon to successfully obtain tuning,
[95], semiconductors and switching,
liquid n
and sensing
crystals properties
[96]. The ultimate goalthat are
is to conducted
successfully by arranging
obtain the functional
tuning, switching, matter on
nonlinear and
sensing properties that are conducted by arranging the functional matter
wavelength level. Moreover, metadevices such as mechanical metadisplay, micro on the subwave-
length level. Moreover, metadevices such as mechanical metadisplay, microelectricity,
ity, acoustics and metadisplays are also emerging and involving nonlinear and q
acoustics and metadisplays are also emerging and involving nonlinear and quantum su-
superconductors,
perconductors, electrostatic
electrostatic and optomechanical
and optomechanical forces and
forces and nonlinear nonlinear
metadevices metadevi
with
nonlinear
nonlinear lumped
lumped components
components [97–100].
[97–100].
Figure
Figure 8. Schematic
8. Schematic of theofNanoengineered
the Nanoengineered Metamaterials
Metamaterials and
and Super Cell. Super Cell.
5.1. Tunable and Reconfigurable Metadevices

5.1. Tunable and Reconfigurable Metadevices
Active metamaterial that is tuning its electromagnetic properties can be achieved by
Active
processing metamaterial
the size, shape and thethat is tuningand
composition, itsby
electromagnetic properties
modifying the near-field can be ach
interaction
processing
between the size,
individual shape and
meta-atoms the composition,
or metamolecule and[101].
resonators by modifying
Reconfigurabletheand
near-field
tunable metadevices can be classified as (i) electrically tunable metasurfaces
tion between individual meta-atoms or metamolecule resonators [101]. Reconf (ETMs) [4],
(ii) mechanically switchable metasurfaces (MSMs) [102], (iii) optically tunable metasurfaces
and tunable metadevices can be classified as (i) electrically tunable metasurfaces
(OTMs) [103], (iv) thermally tunable surfaces (TTMs) [97,103] and finally, (v) chemically
[4], (ii) mechanically
tunable/reconfigurable switchable
metasurfaces metasurfaces
[104,105], (MSMs)
as presented in Figure 9. [102], (iii) optically
metasurfaces (OTMs) [103], (iv) thermally tunable surfaces (TTMs)[97,103] and fin
chemically tunable/reconfigurable metasurfaces [104,105], as presented in Figure
Initially, by using transmission lines tuning, MEMSs have been utilized for
magnetic metamaterials. Similarly, infrared and terahertz detectors for therma
vated structures can be applied. The strength of the dipole–dipole coupling
MEMEs can be continuously adjusted by fine-tuning the distance between the tw
using the MEMS’ actuators, thereby enabling efficient electromagnetic adaptati
tion. The reconfiguration of the metamolecules may enable the polarization of ani
metamaterial to be switched independently [106–109].
Nanomaterials 2022,
Nanomaterials 12, 1027
2022, 12, x FOR PEER REVIEW 12 33
12 of of 32
Figure
Figure9. 9.Reconfigurable
Reconfigurable and
and Tunable
Tunable Metadevices (A,B)Reprinted
Metadevices (A,B) Reprintedwith
withpermission
permission from
from John
John
Wiley and Sons in Copyrights Clearance
Wiley and Sons in Copyrights Clearance center, (C) Reprinted with permission from Copyright
(C) Reprinted with permission from Copyright © ©
2020, American Chemical Society, (D) Reprinted with permission from Creative Commons
2020, American Chemical Society, (D) Reprinted with permission from Creative Commons Attri- Attrib-
ution 4.0 International License, (E) Reprinted with permission from Copyright © 2020, American
bution 4.0 International License, (E) Reprinted with permission from Copyright © 2020, American
Chemical Society.
Chemical Society.
There is consequently a significant impact on metadevices based on MEMS, NEMS,
Initially, by using transmission lines tuning, MEMSs have been utilized for electro-
and micro-/nanofluidic technologies, where the mechanical nanoscale oscillation frequen-
magnetic metamaterials. Similarly, infrared and terahertz detectors for thermally activated
cies could lie within the GHz range, and the metamolecules can be operated at high band-
structures can be applied. The strength of the dipole–dipole coupling of these MEMEs
width on the basis of subwavelength cantilevers.
can be continuously adjusted by fine-tuning the distance between the two rings using the
MEMS’ actuators, thereby
5.2. Electro-Optical enabling efficient electromagnetic adaptation reaction. The recon-
Metadevices
figuration of the metamolecules may enable the polarization of anisotropic metamaterial to
The main advantage of the electro-optical metadevices is their capability of reaching
be switched independently [106–109].
subwavelength deep modulation. They can operate at lower voltages offering an econom-
There is consequently a significant impact on metadevices based on MEMS, NEMS, and
ical benefit compared with conventional technologies that use massive and costly electro-
micro-/nanofluidic technologies, where the mechanical nanoscale oscillation frequencies
optical crystals. Initially, an active metadevice for the terahertz part of the spectrum was
could lie within the GHz range, and the metamolecules can be operated at high bandwidth
developed for a real-time radiation control using electric signals [110]. On a semiconduct-
on the basis of subwavelength cantilevers.
ing substrate, Au metamaterial-arrayed metadevices were successfully fabricated to a
manufactured electro-optical metadevice. An effective Schottky diode was formed by
5.2. Electro-Optical Metadevices
combining Au array and the substrate, in which the semiconducting nature can be con-
The by
trolled main advantage
injected of the electro-optical
and depleted metadevices electrical
carriers. The high-frequency is their capability of reaching
conductivity of the
subwavelength deep modulation. They can operate at lower voltages offering
metamaterial is affected by an electrical signal and impacts its resonant response [111– an eco-
nomical benefit compared with conventional technologies that use massive
113]. This approach offers the possibility to modulate the terahertz transmission by about and costly
electro-optical crystals. Initially, an active metadevice for the terahertz part
50%. The frequency and modulation bandwidths of this kind of metamaterial device are of the spectrum
wasupdeveloped
to 10 MHz for a real-time radiation control using electric signals [110]. On a semicon-
[92,112,114].
ducting substrate, Au
Graphene was also metamaterial-arrayed
extensively used to metadevices were successfully
build electro-optical fabricated
metamaterials (Figure to
a manufactured
10), and successfully applied as a modulator by modifying the electromagnetic responseby
electro-optical metadevice. An effective Schottky diode was formed
combining
particularlyAuinarray and theand
the infrared substrate,
terahertzindomains
which the semiconducting
[115–117]. Significant nature canampli-
oscillator be con-
trolled bythe
tude of injected and depleted
graphene carriers. The
plasmon resonances high-frequency
lead electrical
to noticeable optical conductivity
absorption peaksofatthe
metamaterial is affected Moreover,
the room temperature. by an electrical signal and
the response impacts
of the its resonant
graphene response
can be tuned [111–113].
efficiently by
This approachdoping
electrostatic offers the
overpossibility to modulate
a broad frequency in thethe terahertz
terahertz transmission by about 50%.
range.
The frequency and modulation bandwidths of this kind of metamaterial device are up to
10 MHz [92,112,114].
Graphene was also extensively used to build electro-optical metamaterials (Figure 10),
and successfully applied as a modulator by modifying the electromagnetic response par-
ticularly in the infrared and terahertz domains [115–117]. Significant oscillator amplitude
of the graphene plasmon resonances lead to noticeable optical absorption peaks13atofthe
Nanomaterials 2022, 12, x FOR PEER REVIEW 33
room temperature. Moreover, the response of the graphene can be tuned efficiently by
electrostatic doping over a broad frequency in the terahertz range.
Figure 10. (A). Metamaterial electro-optic switch: (a) A hybrid device with planar plasmonics Au
Figure 10. (A). Metamaterial electro-optic switch: (a) A hybrid device with planar plasmonics Au
metamaterial coated with GLS chalcogenide glass on a SiN membrane. (b) Before GLS deposition,
metamaterial coated with GLS chalcogenide glass on a SiN membrane. (b) Before GLS deposition,
SEM of the asymmetric split-ring ASR slit array. (c) ASR structure computed optical absorption
SEM of without
spectra the asymmetric
GLS film.split-ring
Inside the ASR slit (c),
figure array.
the (c) ASR
black structure
plot labeled computed
i: with GLSoptical absorption
flat film, the blue
plot labeled ii: when the GLS also fills the slits in the gold; the red plot labeled iii: solid andfilm,
spectra without GLS film. Inside the figure (c), the black plot labeled i: with GLS flat the
dashed
blue plot
lines referlabeled ii: when
to the GLS phasestheofGLS also fills A
amorphous the slits
and in the gold;
crystalline the red plot labeled
C, respectively. iii: solid
(Reprinted and
with per-
dashed lines
mission withrefer to the
Rights GLS phases
managed by AIP of amorphous
Publishing)A(B). andElectro-optic
crystalline C,behavior
respectively. (Reprinted
of the with
graphic flake
display:
permissionin positive NLCmanaged
with Rights (a,b) andby (c,d)
AIPinPublishing)
negative NLC, (B). before and after
Electro-optic applying
behavior an graphic
of the electric field.
flake
(e,f) Showing
display: the reorientation
in positive NLC (a,b) and of a (c,d)
graphitic flake inNLC,
in negative the negative dielectric
before and anisotropy
after applying anLC as a result
electric field.
of theShowing
(e,f) appliedtheelectric field (Reprinted
reorientation with permission
of a graphitic flake in the from OSAdielectric
negative Publishing).
anisotropy LC as a result
of the applied electric field (Reprinted with permission from OSA Publishing).
5.3. Phase-Change Metadevices
5.3. Phase-Change
For decades,Metadevices
semiconductor chalcogenide functionality has been used on optical
disksFor decades, semiconductor
supported by a change from chalcogenide
amorphous functionality has been
to crystalline used of
phases on aoptical disks
rewritable
supportedfunction.
memory by a change
Thefrom amorphous
features to crystalline
of polymorphic metalsphases
alsoof a rewritable
provide memory
a method function.
of obtaining
The featuresfast
nanoscale, of polymorphic
and energy-saving metals optical
also provide a method of
and plasmonic obtainingdevices
switching nanoscale, fast and
during this
energy-saving
phase change.optical and plasmonic
The changes switching
are dependent ondevices during this phase change.regime
the stimulation/containment The changes
of the
are dependent
medium, and mayon the
be stimulation/containment
either reversible or irreversibleregime[96].of the medium,
Within an Aland may benonlin-
network, either
reversible or irreversible [96]. Within an Al network, nonlinear optical
ear optical and nonlinear plasmon nanocomposite material were developed through the and nonlinear plasmon
nanocompositeofmaterial
introduction were developed
grain-boundary galliumthrough
(Ga) the introduction
[118,119]. In this of grain-boundary gallium
context, two different
(Ga)
phases[118,119].
of gallium In this context, two
intermediate different triggered
coexistence phases of constant
gallium intermediate
and reversible coexistence
changes.
triggered
This constant
optical and reversible changes.
and temperature-sensitive This optical
composite and temperature-sensitive
metamaterial, composite
formulates a mirror-like
metamaterial,
interface formulates
to silica a mirror-like
and exhibits interface
an extremely to silica and
broadband exhibits anresponse
transitional extremelytobroadband
an optical
transitional response
excitement [2,120,121]. to an optical excitement [2,120,121].
Figure 11
Figure 11 shows
shows aa conceptual
conceptualillustration
illustrationofofmultistate
multistateswitchable
switchablephotonic
photonicspin–orbit
spin–or-
interactions that enable the conversion of various types of spin angular
bit interactions that enable the conversion of various types of spin angular momentum momentum (SAM)
and orbital angular momentum (OAM) by controlling the level
(SAM) and orbital angular momentum (OAM) by controlling the level of crystallization of crystallization of the
Gethe
of 2 Sb2Ge
Te25Sb
alloy (GST) [122]. In symmetric and asymmetric modes, pseudo and real data can
2Te5 alloy (GST) [122]. In symmetric and asymmetric modes, pseudo and real
be coded, in conjunction
data can be coded, in conjunction with the degree
with theof spin freedom.
degree of spinThe metasurfaces
freedom. are interpreted
The metasurfaces are
interpreted in the amorphous state by a simple geometric phase (Pancharatnam–Berry
phase) [123], which leads to symmetrical SAM-to-OAM convert. A suitable stimulus is
needed to interpret the accurate information to excite the GST phase transition from the
amorphous to semi-crystalline state. Therefore, along with the geometric phase, a propa-
in the amorphous state by a simple geometric phase (Pancharatnam–Berry phase) [123],

which leads to symmetrical SAM-to-OAM convert. A suitable stimulus is needed to
interpret the accurate information to excite the GST phase transition from the amorphous
to semi-crystalline state. Therefore, along with the geometric phase, a propagation phase is
Nanomaterials 2022, 12, x FOR PEERalso introduced. The coupling of the two distinct phases enables the two opposite spin
REVIEW 14 ofstates
33
to be regulated independently [124–126]. Two spin states at a given level of crystallization
can be generated in the asymmetric mode. Several additional states of photonic spin–orbit
interactions
of photonic(PSOIs) caninteractions
spin–orbit be recognized by optimizing
(PSOIs) the crystallization
can be recognized by optimizinglevels [127–129].
the crystalli-
Furthermore,
zation levels the PSOIs Furthermore,
[127–129]. which is multistate switchable,
the PSOIs which is have moreswitchable,
multistate information encryption
have more
freedoms and higher security. In addition, while several studies have also confirmed
information encryption freedoms and higher security. In addition, while several studies GST’s
tremendous possibilities in active 1D wave-front modulation, such approaches are
have also confirmed GST’s tremendous possibilities in active 1D wave-front modulation, deduced
mostly from discontinuity
such approaches of themostly
are deduced wave-front
from propagation
discontinuityphase
of theand have no propagation
wave-front link with SAM
and OAM [91,93,130].
phase and have no link with SAM and OAM [91,93,130].
Figure11.11.(A).
Figure The
(A). active
The SAM-to-OAM
active SAM-to-OAM schematic
schematicconversion
conversion schematic
schematic activated with
activated thethe
with suggested
sug-
gested metasurface
metasurface phase change.
phase change. The crystallization
The crystallization level oflevel
GSTofcan
GSTbecan be changed
changed amongamong
thesethese
threethree
modes.
modes.
(B). (B).fabricated
(a) The (a) The fabricated converter’s
converter’s SEM images.
SEM images. (b–d)(b–d) Diffraction
Diffraction patterns
patterns under
under RCPRCP (top)and
(top)
and LCP (bottom) illuminating at various crystallization stages. (e,f) Interference patterns generated
LCP (bottom) illuminating at various crystallization stages. (e,f) Interference patterns generated by
by interference with the OAM beams shown in (b,c) and the titled Gaussian beam, which is circu-
interference with(Reprinted
larly polarized the OAM beams shown in from
with permission (b,c) and
Johnthe titled
Wiley Gaussian
and Sons and beam, whichClearance
Copyright is circularly
polarized
Center). (Reprinted with permission from John Wiley and Sons and Copyright Clearance Center).
5.4. Ultrafast Photonic Metadevices

5.4. Ultrafast Photonic Metadevices
InInsuch
suchdevices,
devices,metallic nanostructuredmetamaterials
metallic nanostructured metamaterialscombinedcombined with
with nonlinear
nonlinear andand
tunable dielectric or semiconductor films and handled by optically
tunable dielectric or semiconductor films and handled by optically ultrafast pulses, offer ultrafast pulses, offer
extremely faster switching as compared to NEMS/MEMS. Intense
extremely faster switching as compared to NEMS/MEMS. Intense light impacting the plas- light impacting the plas-
mon spectrum of a nanostructure triggers variations in the refractive
mon spectrum of a nanostructure triggers variations in the refractive index or absorption index or absorption
ininthe
thelayer
layer next
next to to aaplasmonic
plasmonicmetamaterial
metamaterial array.
array. It may
It may contribute
contribute to a significant
to a significant im-
improvement in the hybrid’s resonant transmission and reflection.
provement in the hybrid’s resonant transmission and reflection. The main candidates The main candidates areare
semiconductors
semiconductorsand andsemiconductor multi-quantumwell
semiconductor multi-quantum wellstructures,
structures, graphene
graphene andand carbon
carbon
nanotubes
nanotubes[131][131]embedded
embedded in in the
the metamaterial’s
metamaterial’s fabric fabric[132].
[132].
The
Theinteraction
interactionbetween
betweenultrafast
ultrafastoptical
opticalpulses
pulses andand metamaterials
metamaterials was first studiedstudied in
order to see
in order to whether
see whether theythey
could modulate
could modulate their terahertz
their terahertz responses
responses optically:
optically:shunting
shuntingthe
metal split-ring
the metal network
split-ring capacitive
network region
capacitive by inserting
region optical
by inserting carriers
optical into into
carriers the supporting
the sup-
ErAs/GaAs superlattice
porting ErAs/GaAs which recovery
superlattice time at the
which recovery ps at
time scale
thecauses
ps scalea profound modulation
causes a profound
ofmodulation
the terahertz of transmission
the terahertz properties
transmission of properties
the planar of metamaterial [133,134]. Advancement
the planar metamaterial [133,134].
inAdvancement in the fieldresonance
the field of plasmonic of plasmonic dueresonance due to metamaterial
to metamaterial network cannetwork can be in
be employed
employed
the in the
optical part ofoptical part of the
the spectrum spectrumthe
to increase to increase
nonlinear theresponse
nonlinearofresponse
the nearby of the
layer
ofnearby layer of the semiconductor
the semiconductor or dielectric.orFano-type
dielectric. resonances
Fano-type resonances
are promotedare promoted by a
by a plasmonic
plasmonic nanostructure,
nanostructure, where more where than a more thanincrease
ten times a ten times increase
of the of the nonlinearity
nonlinearity has
has been achieved.
been achieved. This technique permits the engineering of the nonlinearity of graphene at
a predefined wavelength within a wide range of wavelengths, allowing for optical switch-
ing and pulse shaping applications [135–137].
Kumar et al. [5] recently reported a simple ultrafast THz photonic device where 2D
perovskites and THz metamaterial were combined together for achieving enhanced THz
This technique permits the engineering of the nonlinearity of graphene at a predefined

wavelength within a wide range of wavelengths, allowing for optical switching and pulse
shaping applications [135–137].
Kumar et al. [5] recently reported a simple ultrafast THz photonic device where 2D per-
waves modulation
ovskites (Figure 12).
and THz metamaterial Time-resolved
were THz spectroscopy
combined together for achieving(TRTS)
enhanced measurement
THz waves
technique was
modulation used12).
(Figure to investigate the free
Time-resolved THzcarriers and excitons
spectroscopy (TRTS) dynamics
measurementin atechnique
pure thin
was used to investigate the free carriers and excitons dynamics in a pure thin film ofTHz
film of 2D perovskite. In addition, by spin coating this 2D perovskite thin film onto 2D
metamaterials
perovskite. resonators,
In addition, an ultrafast
by spin active
coating this 2D metadevice for film
perovskite thin THzonto
applications was fabri-
THz metamaterials
cated.
resonators, an ultrafast active metadevice for THz applications was fabricated.
Figure 12. Two-dimensional perovskite ultrafast measurement of. (A) Three-dimensional perov-
Figure 12. Two-dimensional perovskite ultrafast measurement of. (A) Three-dimensional perovskite
skite (black solid curve), mixed 3D–2D perovskite (red solid curve), and pure 2D perovskite (blue
(black solid curve), mixed 3D–2D perovskite (red solid curve), and pure 2D perovskite (blue solid
solid curve) thin films free carrier excitation and relaxation dynamics. Using a 400 nm pump beam
curve) thin films
at 750 μJ/cm 2, thinfree carrier
films excitation and
are photoexcited. (B)relaxation dynamics.
Two-dimensional Using a crystal
perovskite 400 nmstructure’s
pump beam at
sche-
750 µJ/cm 2 , thin films are photoexcited. (B) Two-dimensional perovskite crystal structure’s schematic
matic that makes QWs. (C) Scheme of the quantum confining of the pure 2D perovskite in the QW
that makes(D)
structure QWs. The(C) Schemeexample
artistical of the quantum confining of the pure
of the perovskite-coated 2D perovskite
hybrid metadevicein the
withQW structure
spin-coated
2D The
(D) perovskite
artistical (thickness
example of 60the
nm) on top of TASRhybrid
perovskite-coated and photo-excited withspin-coated
metadevice with a 400 THz 2Doptical pump
perovskite
beam. (E) THz electric field transmission (blue solid line) and THz photomodulation
(thickness 60 nm) on top of TASR and photo-excited with a 400 THz optical pump beam. (E) THz pulse ΔE(t) at
τpump = 1.5 ps (red solid curve) and 20 ps (green solid line) measured in the 2D perovskite
electric field transmission (blue solid line) and THz photomodulation pulse ∆E(t) at τpump = 1.5 ps thin film
(Reprinted with permission from Creative Commons Attribution-Non Commercial License 4.0 (CC
(red solid curve) and 20 ps (green solid line) measured in the 2D perovskite thin film (Reprinted with
BY-NC)).
permission from Creative Commons Attribution-Non Commercial License 4.0 (CC BY-NC)).
5.5. Nonlinear
5.5. Nonlinear Metadevices
Metadevices with
with Varactors
Varactors
By exploiting
By exploiting the
the nonlinear
nonlinear behavior
behavior ofof lumped
lumped elements
elements incorporated into LHMs,
metamaterials can
metamaterials can be
betailored.
tailored.Analogous
Analogous approaches
approaches have been
have developed
been developed for other met-
for other
amaterial systems.
metamaterial ForFor
systems. instance, if positioned
instance, if positionedatata amaximum
maximumpoint pointininthe
the electrical
electrical field,
split-ring metamolecule
split-ring metamolecule resonance can be modified by the the addition
addition ofof aa series
series varactor
varactor
diode with
diode with the
the resonator
resonator distributed
distributed capacitance.
capacitance. A split
split ring
ring with
with embedded
embedded varactor
varactor
presentssecond-
presents second-andandthird-order
third-order nonlinearity
nonlinearity at low
at low powers,
powers, whilewhile the nonlinear
the nonlinear response re-
becomes multivalued
sponse becomes or bistable
multivalued at higher
or bistable powers.
at higher In Figure
powers. 13, a nonlinear
In Figure operating
13, a nonlinear oper-
magnetic metamaterial
ating magnetic is shown.
metamaterial For obtaining
is shown. the tunability
For obtaining of metamaterials
the tunability of metamaterials in a in
mi-a
crowave
microwave domain,
domain,positive-intrinsic-negative
positive-intrinsic-negative (PIN) diodes
(PIN) or varactors
diodes are usually
or varactors inserted
are usually in-
into
sertedtheinto
passive particles
the passive compared
particles to different
compared tuning tuning
to different materials studiedstudied
materials in terahertz
in te-
range [113,138–140]. A tunable metamaterial absorber was suggested
rahertz range [113,138–140]. A tunable metamaterial absorber was suggested by by Zhao etZhao
al. [60]
et
using
al. [60]varactor diode and
using varactor diode theand
proposed absorber
the proposed tunability
absorber was confirmed
tunability was confirmedby 1.5by GHz
1.5
GHz bandwidth measurements. Figure 13A shows the designed tunable metamaterial,
which illustrates the structure of the particle wherein two similar electric-field-coupled-
LC (ELC) spots are printed with same orientation on the substrate. Two ELCs are con-
nected via varactor diode. As the structure resonant frequency is assessed using varactor
bandwidth measurements. Figure 13A shows the designed tunable metamaterial, which 16 of 3
Nanomaterials 2022, 12, x FOR PEER REVIEW
illustrates the structure of the particle wherein two similar electric-field-coupled-LC (ELC)
spots are printed with same orientation on the substrate. Two ELCs are connected via
varactor diode. As the structure resonant frequency is assessed using varactor diode lump
diode lumpunder
parameters, parameters,
different under
reversedifferent reverse
bias voltages bias voltages
the absorption the absorption
frequency frequency o
of the particle
the particle
keeps keeps on
on changing. Onchanging. Onbottom,
the substrate the substrate bottom,
the feeding the feeding
networks networks
are printed are printed
and are
and are used to communicate varactor diodes and feeding lines through
used to communicate varactor diodes and feeding lines through holes. Figure 13C shows holes. Figure 13C
the results
shows theofresults
the experiments as the biasas
of the experiments voltage varies
the bias from varies
voltage 0 to 19from
V, more
0 tothan 90%
19 V, more than
absorption rate with
90% absorption thewith
rate bandwidth 1.5 GHz from
the bandwidth 4.35 to
1.5 GHz 5.85 4.35
from GHzto is 5.85
achieved.
GHz is achieved.
Figure13.
Figure 13.(A)
(A) Proposed
Proposed metamaterial
metamaterial particle’s
particle’s structure.
structure. (B) Fabricated
(B) Fabricated sample
sample front front
view and view
the and th
varactordiodes
varactor diodes feed
feed network.
network. (C) (C) Absorption
Absorption rates rates at different
at different reversereverse bias voltages
bias voltages from 0 tofrom
19 V. 0 to 19 V
(Reprinted
(Reprinted under
under thethe Creative
Creative Commons
Commons Attribution
Attribution 3.0 license).
3.0 license).
6. Photonic Band Gap

6. Photonic Band Gap
Photonic band gap (PBG) materials are artificial periodic structures in one, two, and
Photonic band gap (PBG) materials are artificial periodic structures in one, two, and
three dimensions (1D, 2D, and 3D) with periods that are comparable with the wavelengths
three
of dimensionswaves
electromagnetic (1D, 2D,
(EMWs)and [141,142].
3D) with The
periods
effectthat
of a are comparable
photonic band gap with the wavelength
is quantified
of electromagnetic waves (EMWs) [141,142]. The effect of a photonic band
in terms of the local density of states, which describes the number of available electro- gap is quanti
fied in terms
magnetic modes ofinthe localphotons
which densitymay
of states, which
be emitted describes
at the locationthe number
of the emitterof[143].
available
It elec
tromagnetic
contains modesrange
a prohibited in which photons
of energy causedmay be emitted
by variation atrefractive
in the the location ofinthe
index, emitter
which it [143]
can transmit light
It contains of a specificrange
a prohibited frequency and make
of energy it ideal
caused byforvariation
light harvesting
in the applications,
refractive index, in
which it can transmit light of a specific frequency and make it ideal for light harvestin
applications, as shown in Figure 14. One can customize a structure’s specific band gap b
replicating the periodicity of photonic crystals by establishing a pattern with repetitiv
domains, usually holes in a hexagonal or square structure that alternates between high
as shown in Figure 14. One can customize a structure’s specific band gap by replicating the
periodicity of photonic crystals by establishing a pattern with repetitive domains, usually
holes in a hexagonal or square structure that alternates between high and low dielectric
constant materials.
Figure 14. Representation

Representationofofthe
thephotonic
photonic band
band gap
gap sample
sample (yellow
(yellow colored
colored area)area) onphotonic
on the the photonic
band
band diagram. The different directions along the crystal lattice indicated by the letters along the x-
diagram. The different directions along the crystal lattice indicated by the letters along the x-axis [144]
axis [144] (Reprinted with permission from Creative Commons Attribution-NonCommercial-
(Reprinted with permission from Creative Commons Attribution-NonCommercial-ShareAlike 3.0 license.).
ShareAlike 3.0 license.).
Photonic crystals (PCs) are materials that are periodically distributed in one, two
Photonic
or three spatial crystals (PCs)showing
directions, are materials that are
stop bands orperiodically
photonic band distributed
gaps (PBGs) in one, two or
[141,145].
three spatial directions, showing stop bands or photonic band
The EMWs cannot propagate through the structure, with frequencies falling within PBG.gaps (PBGs) [141,145]. The
EMWs cannotthe
In the PBGs, propagate
localized through
states can the structure,
be createdwith frequencies
by inserting falling
defects intowithin PBG. In
the periodic
the PBGs, the
structures. PCslocalized
have beenstatesintensively
can be created by inserting
investigated, duedefects
to theirinto the periodic
ability to control struc-
the
tures. PCs have
propagation been and
of light intensively investigated,
for the possibility of due
many to new
theiroptical
ability devices.
to controlIfthe thepropaga-
PBG can
tion of an
reflect light and forofthe
incident EMpossibility
waves atof anymany new
angle withoptical
any devices. If thean
polarization, PBG can reflect an
omnidirectional
incident
band gapof(OBG) EM waves within at any angle frequency
a specific with any polarization,
range can beanobtained
omnidirectional band gap
with insignificant
loss [142–147].
(OBG) Fink et frequency
within a specific al. [143] pointed
range canout be
in obtained
1998 thatwith one-dimensional
insignificant loss PCs[142,143–
(1DPCs)
may have
147]. Fink et OBGs, andpointed
al. [143] the general
out in conditions
1998 that for obtaining OBGs
one-dimensional PCsare in 1DPCs.
(1DPCs) may Since
have
then, many
OBGs, and scientists
the general have drawn great
conditions for interest
obtainingfromOBGsthe OBGs
are inin1DPCs.
the 1DPCs Since[146,148–153].
then, many
Such an OBG
scientists haveisdrawn
knowngreatto have potential
interest from applications
the OBGs in [154,155],
the 1DPCssuch as omnidirectional
[146,148–153]. Such an
terahertz
OBG mirrors
is known [156],potential
to have controllable switching[154,155],
applications [157], tunable
such aspolarizer [158], narrowband
omnidirectional terahertz
filters [3][156],
mirrors and optical refractometric
controllable sensingtunable
switching.[157], [159]. OBG width
polarizer plays
[158], an important
narrowband role[3]
filters in
1DPC omnidirectional reflector applications. However, the width
and optical refractometric sensing [159]. OBG width plays an important role in 1DPC om- of the OBGs is usually
narrow in thereflector
nidirectional one-dimensional binary
applications. photonicthe
However, crystals
width(1DBPCs)
of the OBGs formed by twonarrow
is usually different
in
dielectric
the or metal-dielectric
one-dimensional binary composites,
photonic crystals making those structures
(1DBPCs) formed by inefficient
two differentas totaldielectric
reflector
mirrors
or in application,
metal-dielectric as shownmaking
composites, in Figurethose
15. Some methods
structures have been
inefficient as proposed
total reflectorto extend
mir-
the frequency range of OBGs, such as increasing the contrast of
rors in application, as shown in Figure 15. Some methods have been proposed to extend dielectric functions among
PC frequency
the compositesrange [143,146], using
of OBGs, a chirped
such PC [160]
as increasing theorcontrast
photonic heterostructures
of dielectric functions [161–163],
among
or introducing the disorder into periodic structures [164,165]. Additionally,
PC composites [143,146], using a chirped PC [160] or photonic heterostructures [161–163], being put
forward in recent years is one-dimensional ternary photonic crystals (1DTPCs)
or introducing the disorder into periodic structures [164,165]. Additionally, being put for- to obtain the
extended OBGs [166–171]. 1DTPCs comprise three layers of material
ward in recent years is one-dimensional ternary photonic crystals (1DTPCs) to obtain the over a lattice period.
Awasthi etOBGs
extended al. [168] demonstrated
[166–171]. 1DTPCsthat when three
comprise the structure
layers ofwas modified
material overby sandwiching
a lattice period.
a thin layer of ZrO 2 between each two layers, the wavelength
Awasthi et al. [168] demonstrated that when the structure was modified by sandwiching range of OBGs can be
a thin layer of ZrO2 between each two layers, the wavelength range of OBGs can metal-
increased by 108 nm. Wu et al. [170] have shown that the OBGs in the ternary be in-
dielectric PC can be significantly enlarged. Xiang et al. [167] found that sandwiching the
creased by 108 nm. Wu et al. [170] have shown that the OBGs in the ternary metal-dielec-
third material between the two single negative materials enlarge the zero-effective-phase
tric PC can be significantly enlarged. Xiang et al. [167] found that sandwiching the third
bandgap. Kong et al. [171] introduced an OBG on 1D ternary plasma PC. In addition,
material between the two single negative materials enlarge the zero-effective-phase
some 1DTPC-based applications are the tunable optical filter [169] and optical sensing
bandgap. Kong et al. [171] introduced an OBG on 1D ternary plasma PC. In addition, some
device [151].
1DTPC-based applications are the tunable optical filter [169] and optical sensing device
[151].
Nanomaterials 2022,
Nanomaterials 12,12,x 1027
2022, FOR PEER REVIEW 18 of 32 18 of 33
Figure 15. One-dimensional binary photonic crystal (1DBPCs) (AB)N and one-dimensional ternary
photonic
Figure 15. crystal (ACB)N representation,
One-dimensional binary air iscrystal
photonic the background
(1DBPCs) (Reproduced
(AB)N(AB) courtesy of Theternary
and one-dimensional Electro-
Figure 15. One-dimensional
magnetics Academy).N binary photonic crystal (1DBPCs) N and one-dimensional ternary
photonic crystal
photonic crystal(ACB)
(ACB)Nrepresentation, air air
representation, is the background
is the (Reproduced
background courtesy
(Reproduced of The Electro-
courtesy of The Electro-
magnetics Academy).
magnetics Academy).
Photonic Band Gap Materials to Enhance Solar Cell Efficiency
PhotonicTheBand
mostGap Materials
widely usedtopower
Enhance Solar Cell
systems Efficiency
are photovoltaic solar energy conversion ones.
Photonic
However, Band Gap
these Materials
devices are to Enhance
suffering Solar
fromare Cell
relatively Efficiency
a lowsolar
conversion
The most widely used power systems photovoltaic energy efficiency.
conversionThis ones.is
dueThe
However, most
to the these widely
devicesused
wavelength mismatchpower
are suffering systems
between
from the are photovoltaic
narrow
relatively a wavelength solar
low conversion bandenergy conversion
associated
efficiency. with ones.
This
the energy gap in the semiconductor and the wide band of the sun’s
However, these devices are suffering from relatively a low conversion efficiency. This is
is due to the wavelength mismatch between the narrow wavelength(black bandbody) emission
associated
curve.
with
due to The
thethe loss of
energy gap
wavelengthenergy
in the issemiconductor
linked tobetween
mismatch long wavelength
andthethenarrow
widephotons
band with
of theless
wavelength sun’senergy
band(blackstimulat-
body) with
associated
emission
ingenergy
the curve.
the electron’s
gap inThe loss
holes
the of
allenergy
over the
semiconductor is linked
and to
energy long
gap
the wavelength
(i.e.,
wide losingof
band 20% photons
the in with
silicon)
sun’s lessbody)
and
(black energy
photonsemission
stimulating
having shortthe electron’s holes
wavelengths, all overpairs
stimulating the energy
with gap (i.e.,
energy overlosing
the gap20% in losing
(i.e., silicon)32%
andin
curve. The loss of energy is linked to long wavelength photons with less energy stimulat-
photons
silicon).having short wavelengths,
The efficiency stimulating pairs
of the thermophotovoltaic withsystem
(TPV) energymayoverbethe gap (i.e.,bylosing
increased using
ing the electron’s holes all over the energy gap (i.e., losing 20% in silicon) and photons
32% in silicon).
a spectrally The efficiency
dependent coupling of the thermophotovoltaic
between the absorber and (TPV)
the system may bethe
cell to recycle increased
photons
having
by using
with
short
a frequency
wavelengths,
a spectrally dependent
larger
stimulating
than thecoupling
band gap
pairs
between with
frequency
energy over
the absorber and
of the solar
theascell
the
cell,
gap to(i.e.,
shown
losing
recycle the 32% in
in Figure
silicon).
photons
16. The efficiency
with a frequencyoflarger
the thermophotovoltaic
than the band gap frequency (TPV) system maycell,
of the solar be increased
as shown inby using
aFigure
spectrally
16. dependent coupling between the absorber and the cell to recycle the photons
with a frequency larger than the band gap frequency of the solar cell, as shown in Figure
16.
Figure16.
Figure 16.Illustration
Illustrationofofaaconversion
conversionsystem
systemfor
forTPV
TPVenergy.
energy.The
Thethermal
thermalradiation
radiationofofthe
thesun
sunheats
heats
anintermediate
an intermediateabsorber.
absorber.Filter-transmitted
Filter-transmittedradiation
radiationfrom
fromthe
theemitter
emitterilluminate
illuminatethe
thephotovoltaic
photovoltaic
(PV)cell.
(PV) cell.
Figure 16. Illustration of a conversion system for TPV energy. The thermal radiation of the sun heats
an intermediate absorber. Filter-transmitted radiation from the emitter illuminate the photovoltaic
(PV) cell.
In this approach, materials of the specific PBG are designed in such a way to obtain
highly efficient solar cells [141,145]. These are a new class of periodic materials which
enable accurate control of all properties of EMWs [144,172]. A PBG, similar to the electronic
band gap in semiconductor crystals, occurs in a periodic dielectric or metallic media. The
electromagnetic radiation light cannot propagate within the PBG spectral range. Through
the engineering of the photonic dispersion relationship, the ability to tailor the properties
of the electromagnetic radiation in a prescribed way allows the design of systems that
accurately control the emission and absorption of light. This gives rise to new phenomena
including inhibition and enhancement of spontaneous emission [145], strong localiza-
tion of light [141], formation of atom-photon bound states [173], quantum interference
effects in spontaneous emission [174], single atom and collective atomic switching behav-
ior through coherent resonant pumping and atomic reversal without fluctuations [175].
Feng et al. [176] reported the performance improvement of a near-field TVP device by
a back surface reflector. As photonic crystals are the leading candidates for frequency-
and angular-selective radiating elements in TPV devices. Therefore, employment of such
photonic crystal-based angle- and frequency-selective absorbers facilitates a strong en-
hancement of the conversion efficiency of solar cell devices without using concentrators.
The increment in efficiency is different for different materials, strategy (i.e., used as emitter,
absorber or reflector) and temperature of the cell/system. As a matter of fact, using as
back surface reflector (BSF), efficiency increased from 16.4% to 21% and power output has
increased by 10%. Bierman et al. [177] reported for solar TPV, the 6.8% efficiency increase
of the solar-to-electrical by pairing a one-dimensional SI/SiO2 photonic crystal selective
thermal emitter and a tandem plasma-interference optical filter by spectral enhancement.
Bhatt et al. [178] reported a STPV system with the overall conversion efficiency of 8.4% by
using a nanostructure-based spectrally selective emitter/absorber. The spectral properties
of the emitter were optimized to maximize the output power density from the TPV cells.
Changes in the spontaneous emission rate of atoms inside the photonic crystal struc-
ture in turn determine significant changes in thermal radiative processes. Thermal radiation
is simply thermally driven by spontaneous emission and in thermal equilibrium with its
surrounding material. In 1999, Cornelius and Dowling proposed the use of PBG materials
to alter thermal emission [179]. Two alternative approaches were explored: a method
based on a passive lossless PBG thin-film coating over the absorber, and an approach using
an active PBG material made from an absorbent medium. In 2000, the thermal emission
modification was experimentally demonstrated using a thin 3D photonic crystal slab on
a silicon substratum [180]. Pralle et al. [181] used a PBG technique to prove a thermally
excited, narrow-band, mid-infrared source. Recently, researchers at Sandia Labs demon-
strated a high-efficiency TPV system using tungsten photonic crystals [182,183]. These
studies suggest that it is possible to achieve dramatic modifications of Planck’s black body
radiation spectrum by optimizing the coupling of the multi-mode radiation field of a PBG
material and a spatially extended collection of atomic or electronic emitters [179,182]. The
thermal emission of radiation is strongly suppressed in the PBG spectral range, whereas
the thermal emission of radiation is resonantly increased up to the black-body limit for
specific frequencies in the permitted photonic bands which correspond to the transmission
resonances of the photonic crystal.
For important technological applications, such as low-threshold micro-lasers [18,184],
ultra-fast all-optical switches and micro-transistors [185–187], these remarkable phenomena
have attracted considerable interest.
7. Solar Cell Efficiency Enhancement and Negative Refractive Index Materials

In the weak absorption spectral domain, solar cells of planar thin-film configuration
can benefit from resonance of Fabry–Perot to perform more effectively [130,188–190]. Simi-
larly, spectral width significantly reduces for a thicker solar cell and their number increases,
both being disadvantageous. There have been reports that a single Fabry–Perot resonance,
which is spectrally broad, can be obtained from an optically alternate material, namely a
material that has a negative but otherwise similar refractive index to the material of the
solar cell with the same impedance. This is critical for improving the absorption across
the interested spectral domain. Even though, the material assumed with idealistic prop-
erties cannot be obtained; therefore, nanostructures such as photonic crystals engineered
for dispersion, can be manipulated by actual application. Their optical response may be
comparable to the desired within the acceptable spectral range.
In solar cells the photon management contributes to improving spectrally and spatially
the absorption of the incident sunlight [191,192]. This concept was under active investiga-
tion during the last decade. In this respect, numerous advanced micro- and nano-optical
principles have been extended efficaciously to the photovoltaic domain. It usually goes
further than conventional methodologies in which the incident of sunlight is only dis-
persed in macroscopic structures in order to maximize the efficacious path length [193,194].
Concepts used in these new methods are namely photonic crystals [195,196], metallic
nanoparticles [197–199], waveguides [200,201] and diverse nanoshapes [202–204]. In the
end, all these approaches focus on reducing PV material thickness without performance
degradation. This minimizes recombination losses in volume, reduces material usage
and accelerates the deposition time, whereas maintaining the level of absorption remains
sufficiently high. Metamaterial’s field may allow a degree of freedom to work along two
directions, such as properties for a specific structure are assessed and implemented for
other purposes, e.g., to change the local state density [205] or to increase absorption [49,206].
On the other hand, a lot of essential work has been achieved in the opposite direction.
8. Metamaterials and Metasurfaces: Glimpses of New Trends

8.1. Terahertz Metamaterials
Terahertz (THz) radiation in the electromagnetic spectrum with its non-ionizing prop-
erty has the ability to sense materials with an extremely high accuracy. THz devices have
potential applications in diverse areas such as imaging, high-resolution spectroscopy and
biomedical analytics. The idea to realize the optically reconfigurable metasurfaces based on
phase-change material was proposed for multifunctional rewritable metadevices through
laser writing that would open up a new avenue for real application of metamaterials.
However, it is still not possible to realize the real-time control with the optical writing
approach. Metasurfaces have provided a novel route to control the local phase of electro-
magnetic radiation through subwavelength scatterers where the properties of each element
remain passive. A passive metasurface design can only achieve a specific functionality
as it is extremely challenging to reconfigure each element that contributes toward the
control of the radiation. To add more insights to this article, especially with the context
of this planetary pandemic, some works in this particular topic of metamaterials should
be highlighted. Indeed, in the diagnosis of severe contagious diseases there is an urgent
need for protein sensors with large refractive index sensitivities. Current terahertz (THz)
metamaterials cannot be used to develop such protein sensors due to their low refractive
index sensitivities. Silalahi et al. [207] proposed an efficient method based on a patterned
photoresist to float the split-ring resonators (SRRs) of a terahertz metamaterial at a height
of 30 µm from its substrate that is deposited with complementary SRRs, and is compatible
with all geometrical structures of terahertz metamaterials to increase their refractive index
sensitivities. This floating terahertz metamaterial has demonstrated an extremely large
refractive index sensitivity of 532 GHz/RIU and was tested successfully to sense bovine
serum albumin (BSA) and the protein binding of BSA and anti-BSA as BSA, and anti-BSA
solutions with low concentrations that are smaller than 0.150 µmol/L.
On the other hand, anapole metamaterials have recently attracted increasing attention
owing to their unique nonradiating and nontrivial properties. Even though anapole modes
have been demonstrated in metamaterials with three-dimensional structures, the design
and realization of planar anapole metamaterials in a wide frequency range is still a big
challenge. Li et al. [208] proposed and experimentally demonstrated a planar anapole
metamaterial consisting of dumbbell-shaped apertures on a stainless-steel sheet at terahertz
frequencies, and the planar metamaterial was even able to generate a resonant transparency
in the terahertz spectrum due to the excitation of the anapole mode.
Zhang et al. [209] proposed a scheme based on a microelectromechanical system
(MEMS) to reconfigure the resonance and radiation phase via control of each dipolar ele-
ment. The suspension angle of the individual bimorph cantilever in air can be precisely
controlled through electrostatic actuation that determines the operative phase diagram of
the metadevice. The dynamic polarization conversion is demonstrated through global con-
trol. In addition, it is proposed that a multifunctional operation such as dynamic wavefront
deflection and rewritable holographic display can be accomplished by using 1D and 2D con-
trol of the cantilever array when each cantilever in the MEMS metadevice array is uniformly
and accurately controlled in the large-area samples [5]. Such a rewritable proposition can
enable a myriad of applications of MEMS-based metadevices in polarization-division multi-
plexing and dynamic flat lenses. As an alternative, microelectromechanical system (MEMS)
metamaterials have enabled the dynamic control of electromagnetic waves ranging from
microwave to infrared through thermal bimorphs, comb drives, out-of-plane deformable
cantilevers and electrostatically actuated beams [210].
8.2. Chiral Metamaterials

Chiral metamaterials have greatly impacted the field of optical sensing over the past
decade [211,212]. To improve the sensitivity of chiral sensing platforms, enhancing the
chiroptical response is necessary. Metasurfaces, have attracted significant attention because
of their ability to enhance the chiroptical response by manipulating amplitude, phase and
polarization of electromagnetic fields [22]. They can exhibit chiroptical phenomena, such
as the difference in the propagation velocity, known as optical rotatory dispersion (ORD),
and the difference of absorption, known as circular dichroism (CD), between left and right
circularly polarized light [213–215].
The field of chiral plasmonics has met huge progress with machine-learning (ML)-
mediated metamaterial prototyping. Ashalley and coworkers [216] presented an end-to-end
functional bidirectional deep-learning (DL) model for three-dimensional chiral metamate-
rial design and optimization, exploring in detail the nontrivial relationship between the
metamaterials’ geometry and their chiroptical response, eliminating the need for auxiliary
networks or equivalent approaches to stabilize the physically relevant output. This model
efficiently explored the sensing of biomolecular enantiomers and showed a promising
potential to other applications including photodetectors, polarization-resolved imaging
and circular dichroism (CD) spectroscopy.
8.3. Acoustic Metasurfaces

The acoustic metasurfaces field has emerged in recent years and is propelled by
the desire to control the propagation of acoustic waves by compact structures [217]. The
strategy for the design of acoustic metasurfaces depends on the targeted physical properties
and applications (reflection, transmission and/or absorption). In the designs of acoustic
metasurfaces for specific applications, precise control of the phase and amplitude of acoustic
wave propagation is required. A thorough assessment of the design choice should take
place before tackling any specific applications. The main metasurface designs are based on
the Helmholtz resonator-like structure [218], membrane-type structure [219] and coiling-up
space structure [220].
8.4. Bianisotropic Metasurfaces

Metasurfaces which exhibit magnetoelectric coupling are called bianisotropic metasur-
faces [221]. Bianisotropic materials acquire magnetic (electric) polarization when excited
by electric (magnetic) external field. Thus, the term “bianisotropy” implies double (“bi-”)
polarization mechanism and anisotropic response. Optically thin composite layers can be
modeled as electric and magnetic surface current sheets flowing in the layer volume in the
metasurface plane. In the most general linear metasurface, the electric surface current can
be induced by both incident electric and magnetic fields. Likewise, magnetic polarization
and magnetic current can be induced also by external electric field. Bianisotropy is not
always attributed to spatial dispersion. Alternatively, nonreciprocal bianisotropic effects
can be achieved, for example, in composites containing both magnetically and electrically
polarizable components which are coupled via their reactive fields and experience influence
of some external time-odd bias field or force [222–224]. Nonreciprocal bianisotropic meta-
surfaces can be used to design, for instance, various types of isolators with simultaneous
control of amplitude and polarization of transmitted waves [222–224].
8.5. Quantum Photonics Metasurfaces

An increasing interest in bringing novel functionalities enabled by flat photonics to
the realm of quantum optics is recently noticed. Quantum optical technologies require
sources of single photons, entangled photons and other types of nonclassical light, as
well as novel methods of detection [88,185,225]. The quantum states could be based on
different degrees of freedom of light polarization, direction and orbital angular momentum.
Metasurfaces have a real potential for the realization of each of these states. Rapid progress
in the development of metaphotonics allowed bulky optical assemblies to be replaced with
metasurfaces, opening a broad range of novel and superior applications of flat optics to the
generation, manipulation and detection of classical light [226–230].
8.6. Liquid Crystal-Based Metamaterials

Active liquid crystals (LCs)-based metamaterials have been attracting an increasing
amount of attention in the past few years because of their controlled characteristics leading
to emerging applications, including modulators, switches and filters. The use of LCs
allows for the achievement of metadevices with dynamic functions induced by electro-,
magneto-, photo- and temperature-sensitive properties. Kowerdziej et al. [231] reported
on the shortening of switching times of various soft-matter-based tunable metamaterials
to improve the functionality of modern active devices. As a matter of fact, the frequency-
convertible dielectric anisotropy of the dual-frequency mixture has shown to provide the
opportunity to create a fast-response in-plane switching metasurface at the nanoscale,
which could be tuned by an electrical signal with different frequencies [232–234].
8.7. Non-Hermitian Photonics and Metamaterials/Metasurfaces

In quantum mechanics, hermiticity is usually assumed implying a closed system. Her-
mitian systems exhibit energy conservation, real eigenvalues and physically meaningful
observables. If physical systems are allowed to exchange energy with their environments,
these properties are no longer guaranteed. Such open or non-Hermitian systems generally
have complex eigenvalues and may exhibit exceptional points [235–237]. Systems tuned
to an exceptional point are extremely sensitive to perturbations [238,239]. In recent years,
there has been tremendous progress in the theory and experimental implementations of
non-Hermitian photonics, including all-lossy optical systems as well as parity-time sym-
metric systems [236,240]. Parity-time (PT) symmetry is a fascinating concept to make sense
of non-Hermitian Hamiltonians. In particular, non-Hermitian concepts can be translated
to electromagnetic structures by means of spatial modulation of loss and gain, which is
becoming technologically viable in artificial materials and metamaterials [241]. Nowadays,
materials and their geometry make up the tools for designing nanophotonic devices, but
in the past to design the devices, focus used to remain usually on the real part of the
refractive index of materials and the absorption, or imaginary index, was tolerated as an
undesirable effect. However, a clever distribution of imaginary index of materials offers
an additional degree of freedom for designing nanophotonic devices. Such configurations
can be synthesized by establishing an even distribution in the real part of the refractive
index while imposing an antisymmetric gain/loss profile, associated with the imaginary
part of the refractive index [240]. The intrinsic capability of photonics of creating and
superposing non-Hermitian eigenstates through optical gain and loss is ideal for exploring
various non-Hermitian paradigms. PT metamaterials and metasurfaces may operate in

microwave frequencies and higher, suppress losses and provide tunability through the nat-
ural appearance of a transition to a PT-broken phase. These systems enable new pathways
for metasurface design using phase, symmetry and topology as powerful tools [242]. The
research area of non-Hermitian photonics is relatively new and it is still largely unexplored.
Novel theoretical ideas combined with new experimental schemes are expected to produce
more surprising results, leading to altogether different, previously unknown, means for
controlling light-matter interactions both in the classical and the quantum regimes.
8.8. Metamaterials-Based Coherent Perfect Absorber

A coherent perfect absorber is a system in which the complete absorption of electro-
magnetic radiation is achieved by controlling the interference of multiple incident waves.
Interference is a ubiquitous wave phenomenon occurring whenever two or more coherent
waves overlap, leading to a spatial redistribution of energy. Interference underlies the
operation of numerous devices, in optics and photonics concerns the role that interference
has in regulating light absorption. In particular, it is possible for a device to perfectly
absorb an incident electromagnetic wave if all the wave components scattered by the device
destructively interfere. Coherent perfect absorption (CPA) is a multichannel waveform
shaping protocol that leads to the complete extinction of a monochromatic radiation when
it enters a weakly lossy cavity [243,244]. Perfect absorption of light is of great importance in
a variety of applications ranging from sensing to stealth technologies [245,246]. Achieving
perfect absorption at subwavelength scale is particularly important for nanophotonic and
electromagnetic applications. In recent years, various approaches of designing ultrathin
perfect absorbers have been proposed, including thin films, metamaterials and metasur-
faces [247]. However, it was found that the incident energy could be perfectly absorbed
under incidence on opposite sides of an absorber. This interference-assisted absorption is
known as “coherent perfect absorption”, and was experimentally demonstrated in a silicon
slab under coherent monochromatic illumination [243,244,248].
9. Summary
The development of active metasurfaces and metamaterials to replace conventional
optical elements is still in its early stages, although the field of metasurfaces is rather well
established. In this review, we have reported the most recent and most relevant literature
works related to the exciting field of metamaterials. Focus was put on metamaterials
classification, evolution of metasurfaces, emerging metadevices and their mechanism of
functioning. Traditional and new emerging fabrication techniques for metasurfaces are
summarized with their associated advantages and limitations. Similarly, 3D metamaterial
fabrication has been discussed. We have shed light onto photonic band gap tuning via the
use of different metasurfaces to improve the absorption spectrum for specific applications
such as enhancing solar cell efficiency. In photovoltaics, the level of light absorption can be
commonly achieved by reducing the thickness of the absorption layer and minimizing the
recombination losses. We have seen that these recommendations might be achieved through
use of photonic crystals, metallic nanoparticles, waveguides and diverse nanoshapes. Thus,
the door to metamaterials is fully opened now for the achievement of tangible innovative
optoelectronic devices.
Author Contributions: All the authors have equal contributions. A.A. has gathered the relevant
and up-to-date data for preparing the manuscript by arranging the most recent publications. B.A.
conceptualized the idea for preparing the review paper, participated in writing and revised the
manuscript. A.M. has contributed to calculations and write up of the first version of this paper. All
authors have read and agreed to the published version of the manuscript.
Funding: This research is funded by Qatar National Research Fund (A member of Qatar Foundation)
through NPRP grant # NPRP11S-0117-180330.
Conflicts of Interest: The authors declare no conflict of interest.
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Nanomaterials 2022, 12, 1027. https://doi.org/10.3390/nano12061027 https://www.mdpi.com/journal/nanomaterials

2. Classification of Metamaterials According to Their Physical Properties

Nanomaterials 2022, 12, 1027 5 of 32

Nanomaterials 2022, 12, 1027 6 of 32

exploit its inherent line-of-sight depositing characteristics, required metal or dielectric

4.3. Soft Lithography

4.4. Electron Beam Lithography

4.5. Three-Dimensional Metamaterial Fabrication Techniques

Nanomaterials 2022, 12, 1027 11 of 32

5.1. Tunable and Reconfigurable Metadevices

in the amorphous state by a simple geometric phase (Pancharatnam–Berry phase) [123],

5.4. Ultrafast Photonic Metadevices

This technique permits the engineering of the nonlinearity of graphene at a predefined

6. Photonic Band Gap

Figure 14. Representation

7. Solar Cell Efficiency Enhancement and Negative Refractive Index Materials

8. Metamaterials and Metasurfaces: Glimpses of New Trends

8.2. Chiral Metamaterials

8.3. Acoustic Metasurfaces

8.4. Bianisotropic Metasurfaces

8.5. Quantum Photonics Metasurfaces

8.6. Liquid Crystal-Based Metamaterials

8.7. Non-Hermitian Photonics and Metamaterials/Metasurfaces

various non-Hermitian paradigms. PT metamaterials and metasurfaces may operate in

8.8. Metamaterials-Based Coherent Perfect Absorber

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